Edge stabilization in reduced-dimensional perovskites.

Li Na Quan; Dongxin Ma; Yongbiao Zhao; Oleksandr Voznyy; Haifeng Yuan; Eva Bladt; Jun Pan; F Pelayo García de Arquer; Randy Sabatini; Zachary Piontkowski; Abdul-Hamid M. Emwas; Petar Todorović; Rafael Quintero-Bermudez; Grant Walters; James Z Fan; Mengxia Liu; Hairen Tan; Makhsud I Saidaminov; Liang Gao; Yiying Li; Dalaver H. Anjum; Nini Wei; Jiang Tang; David W McCamant; Maarten B J Roeffaers; Sara Bals; Johan Hofkens; Osman Bakr; Zhenghong Lu; E. Sargent

doi:10.1038/s41467-019-13944-2

Edge stabilization in reduced-dimensional perovskites.

Li Na Quan, Dongxin Ma, Yongbiao Zhao, Oleksandr Voznyy, Haifeng Yuan, Eva Bladt, Jun Pan, F Pelayo García de Arquer, Randy Sabatini, Zachary Piontkowski, Abdul-Hamid M. Emwas, Petar Todorović, Rafael Quintero-Bermudez, Grant Walters, James Z Fan, Mengxia Liu, Hairen Tan, Makhsud I Saidaminov, Liang Gao, Yiying LiDalaver H. Anjum, Nini Wei, Jiang Tang, David W McCamant, Maarten B J Roeffaers, Sara Bals, Johan Hofkens, Osman Bakr, Zhenghong Lu, E. Sargent

Research output: Contribution to journal › Article › peer-review

168 Scopus citations

Abstract

Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 ± 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m-2; their maximum luminance is 4.5 × 104 cd m-2 (corresponding to an EQE of 5%); and, at 4000 cd m-2, they achieve an operational half-lifetime of 3.5 h.

Original language	English (US)
Journal	Nature communications
Volume	11
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-13944-2
State	Published - Jan 10 2020

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): KUS-11-009-21
Acknowledgements: This publication is based in part on work supported by an award (KUS-11-009-21) from the King Abdullah University of Science and Technology (KAUST), by the Ontario Research Fund Research Excellence Program, by the Ontario Research Fund (ORF), by the Natural Sciences and Engineering Research Council (NSERC) of Canada, and by the US Department of Navy, Office of Naval Research (Grant Award No. N00014-17-1-2524). H.Y. acknowledges the Research Foundation-Flanders (FWO Vlaanderen) for a postdoctoral fellowship. E.B. gratefully acknowledges financial support by the Research Foundation-Flanders (FWO Vlaanderen). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #815128-REALNANO). M.B.J.R. and J.H. acknowledge the Research Foundation-Flanders (FWO, Grants G.0962.13, G.0B39.15, AKUL/11/14 and G0H6316N), KU Leuven Research Fund (C14/15/053) and the European Research Council under the European Union’s Seventh Framework Programme (FP/2007-2013)/ERC Grant Agreement No. [307523], ERC-Stg LIGHT to M.B.J.R. DFT calculations were performed on the IBM BlueGene Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP). M.I.S. acknowledges the Banting Postdoctoral Fellowship program from the Natural Sciences and Engineering Research Council of Canada (NSERC). H.T. acknowledges the Netherlands Organisation for Scientific Research (NWO) for a Rubicon grant (680-50-1511).

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Quan, L. N., Ma, D., Zhao, Y., Voznyy, O., Yuan, H., Bladt, E., Pan, J., García de Arquer, F. P., Sabatini, R., Piontkowski, Z., Emwas, A.-H. M., Todorović, P., Quintero-Bermudez, R., Walters, G., Fan, J. Z., Liu, M., Tan, H., Saidaminov, M. I., Gao, L., ... Sargent, E. (2020). Edge stabilization in reduced-dimensional perovskites. Nature communications, 11(1). https://doi.org/10.1038/s41467-019-13944-2

@article{718bfa15144646e29e770e1c961fc75f,

title = "Edge stabilization in reduced-dimensional perovskites.",

abstract = "Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 ± 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m-2; their maximum luminance is 4.5 × 104 cd m-2 (corresponding to an EQE of 5%); and, at 4000 cd m-2, they achieve an operational half-lifetime of 3.5 h.",

author = "Quan, {Li Na} and Dongxin Ma and Yongbiao Zhao and Oleksandr Voznyy and Haifeng Yuan and Eva Bladt and Jun Pan and {Garc{\'i}a de Arquer}, {F Pelayo} and Randy Sabatini and Zachary Piontkowski and Emwas, {Abdul-Hamid M.} and Petar Todorovi{\'c} and Rafael Quintero-Bermudez and Grant Walters and Fan, {James Z} and Mengxia Liu and Hairen Tan and Saidaminov, {Makhsud I} and Liang Gao and Yiying Li and Anjum, {Dalaver H.} and Nini Wei and Jiang Tang and McCamant, {David W} and Roeffaers, {Maarten B J} and Sara Bals and Johan Hofkens and Osman Bakr and Zhenghong Lu and E. Sargent",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): KUS-11-009-21 Acknowledgements: This publication is based in part on work supported by an award (KUS-11-009-21) from the King Abdullah University of Science and Technology (KAUST), by the Ontario Research Fund Research Excellence Program, by the Ontario Research Fund (ORF), by the Natural Sciences and Engineering Research Council (NSERC) of Canada, and by the US Department of Navy, Office of Naval Research (Grant Award No. N00014-17-1-2524). H.Y. acknowledges the Research Foundation-Flanders (FWO Vlaanderen) for a postdoctoral fellowship. E.B. gratefully acknowledges financial support by the Research Foundation-Flanders (FWO Vlaanderen). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #815128-REALNANO). M.B.J.R. and J.H. acknowledge the Research Foundation-Flanders (FWO, Grants G.0962.13, G.0B39.15, AKUL/11/14 and G0H6316N), KU Leuven Research Fund (C14/15/053) and the European Research Council under the European Union{\textquoteright}s Seventh Framework Programme (FP/2007-2013)/ERC Grant Agreement No. [307523], ERC-Stg LIGHT to M.B.J.R. DFT calculations were performed on the IBM BlueGene Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP). M.I.S. acknowledges the Banting Postdoctoral Fellowship program from the Natural Sciences and Engineering Research Council of Canada (NSERC). H.T. acknowledges the Netherlands Organisation for Scientific Research (NWO) for a Rubicon grant (680-50-1511).",

year = "2020",

month = jan,

day = "10",

doi = "10.1038/s41467-019-13944-2",

language = "English (US)",

volume = "11",

journal = "Nature communications",

issn = "2041-1723",

publisher = "Nature Research",

number = "1",

}

Quan, LN, Ma, D, Zhao, Y, Voznyy, O, Yuan, H, Bladt, E, Pan, J, García de Arquer, FP, Sabatini, R, Piontkowski, Z, Emwas, A-HM, Todorović, P, Quintero-Bermudez, R, Walters, G, Fan, JZ, Liu, M, Tan, H, Saidaminov, MI, Gao, L, Li, Y, Anjum, DH, Wei, N, Tang, J, McCamant, DW, Roeffaers, MBJ, Bals, S, Hofkens, J, Bakr, O, Lu, Z & Sargent, E 2020, 'Edge stabilization in reduced-dimensional perovskites.', Nature communications, vol. 11, no. 1. https://doi.org/10.1038/s41467-019-13944-2

TY - JOUR

T1 - Edge stabilization in reduced-dimensional perovskites.

AU - Quan, Li Na

AU - Ma, Dongxin

AU - Zhao, Yongbiao

AU - Voznyy, Oleksandr

AU - Yuan, Haifeng

AU - Bladt, Eva

AU - Pan, Jun

AU - García de Arquer, F Pelayo

AU - Sabatini, Randy

AU - Piontkowski, Zachary

AU - Emwas, Abdul-Hamid M.

AU - Todorović, Petar

AU - Quintero-Bermudez, Rafael

AU - Walters, Grant

AU - Fan, James Z

AU - Liu, Mengxia

AU - Tan, Hairen

AU - Saidaminov, Makhsud I

AU - Gao, Liang

AU - Li, Yiying

AU - Anjum, Dalaver H.

AU - Wei, Nini

AU - Tang, Jiang

AU - McCamant, David W

AU - Roeffaers, Maarten B J

AU - Bals, Sara

AU - Hofkens, Johan

AU - Bakr, Osman

AU - Lu, Zhenghong

AU - Sargent, E.

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): KUS-11-009-21 Acknowledgements: This publication is based in part on work supported by an award (KUS-11-009-21) from the King Abdullah University of Science and Technology (KAUST), by the Ontario Research Fund Research Excellence Program, by the Ontario Research Fund (ORF), by the Natural Sciences and Engineering Research Council (NSERC) of Canada, and by the US Department of Navy, Office of Naval Research (Grant Award No. N00014-17-1-2524). H.Y. acknowledges the Research Foundation-Flanders (FWO Vlaanderen) for a postdoctoral fellowship. E.B. gratefully acknowledges financial support by the Research Foundation-Flanders (FWO Vlaanderen). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #815128-REALNANO). M.B.J.R. and J.H. acknowledge the Research Foundation-Flanders (FWO, Grants G.0962.13, G.0B39.15, AKUL/11/14 and G0H6316N), KU Leuven Research Fund (C14/15/053) and the European Research Council under the European Union’s Seventh Framework Programme (FP/2007-2013)/ERC Grant Agreement No. [307523], ERC-Stg LIGHT to M.B.J.R. DFT calculations were performed on the IBM BlueGene Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP). M.I.S. acknowledges the Banting Postdoctoral Fellowship program from the Natural Sciences and Engineering Research Council of Canada (NSERC). H.T. acknowledges the Netherlands Organisation for Scientific Research (NWO) for a Rubicon grant (680-50-1511).

PY - 2020/1/10

Y1 - 2020/1/10

N2 - Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 ± 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m-2; their maximum luminance is 4.5 × 104 cd m-2 (corresponding to an EQE of 5%); and, at 4000 cd m-2, they achieve an operational half-lifetime of 3.5 h.

AB - Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 ± 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m-2; their maximum luminance is 4.5 × 104 cd m-2 (corresponding to an EQE of 5%); and, at 4000 cd m-2, they achieve an operational half-lifetime of 3.5 h.

UR - http://hdl.handle.net/10754/661083

UR - http://www.nature.com/articles/s41467-019-13944-2

UR - http://www.scopus.com/inward/record.url?scp=85077680403&partnerID=8YFLogxK

U2 - 10.1038/s41467-019-13944-2

DO - 10.1038/s41467-019-13944-2

M3 - Article

C2 - 31924790

SN - 2041-1723

VL - 11

JO - Nature communications

JF - Nature communications

IS - 1

ER -

Edge stabilization in reduced-dimensional perovskites.

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